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Annual Reviews

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~
ALPHA RADIOACTIVITY
BY I. PERLMANAND FRANKASARO
Radiation Laboratory and Departmentof Chemistry,
University of California, Berkeley, California

INTRODUCTION
A comparison of the number of a-emitters known at present with those
known a few years ago serves as a rough index of the comparative research
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activity on a-radloactlvlty and associated problems. By 1944 just 26 a-emlt-


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ters had been definitely identified and reported, and of these all but one were
membersof the natural radioactive families. (Some others were found during
the war years but publication was delayed.) In 1948 the total number of
a-emitters had climbed to nearly 90~ and at the end of 1953 there were more
than 160 known. The increase in numbers of a-emltters has been accom-
panied by diversification of the information attainable by the treatment of
a-decay data as well as a better insight into those features of a-radioactivity
already recognized. It is perhaps worth recalling, however, that the basic
a-decay theory (1, 2) was developed in the "days of the natural radioactlvi-
ties" and precise absolute a-energies were determined during this period (3).
The huge increase in numbers of a-emkters is a result of several stimuli.
The wartime military efforts in atomic energy were directly concerned with
several new a-emltters, and as a result of their preparation a number of
others appeared as by-products. This work stimulated the desire to know
the nuclear properties of other isotopes of these elements and developed into
a search for higher transuranium elements as well. It is interesting to note
that at present there are as many elements known above U as there are be-
tween U and Bi. Another important source of a-emltters came with the con-
struction of particle accelerators operating in a new high-energy range. With
the use of such instruments (particularly the Berkeley 184-inch cyclotron),
exploration into the region of neutron deficient isotopes became possible and
resulted in the discovery of a wide range of new a-emitters including a group
among the rare earth elements.
This review will be confined in large measure to the development of a few
topics which have stemmedfrom the investigations of the past several years.
The classical work on a-radioactivity will not be covered, and no special
treatment will be given to the natural a-emitters.
A few brief statements outlining these newer developments are given in
the following:
(a) Regularities in a-decay energy.--It is possible to correlate decay
energies on a seml-emplrical basis, and the observed regularities make it
possible to predict rather closely the decay energies of unknownspecies.
1 The survey of the literature pertaining to this review was concludedin April,
1954.
157
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i58 PERLMAN AND ASARO

(b) Regularities of decay lifetlmes.--It is now known that one-body


decay theory, not far different in form from that originally proposed, is
capable of yielding precise lifetime values for most even-even nuclei but not
for other types. Lifetimes can be predicted on a semi-empirical basis for al-
most all eases.
(c) Newdevelopments in a-decay theory.--The results to be cited on odd
nucleon types and on the complex spectra of all types serve to delimit the
applicability of present a-decay theory and to define the problems which
must be solved by a more comprehensive theory. Some attempts to build
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upon the classical theory will be mentioned.


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(d) Spectroscopic states deduced from alpha decay.--Almost all a-emit-


ters show complex spectra when examined with instruments of high resolu-
tion. The mapping of nuclear spectroscopic states populated in the a-decay
process has yielded substantial information on the general picture of energy
levels in the heavy element region.
Unfortunately, it will not be possible in this review to discuss the impor-
tant advances in detection and energy determination of a-particles. Also
omitted are the means for producing the many a-emitters and any individual
discussion of many of the interesting new species.

ALPI~IA DI~CAY ENE;RGY

Somewhat beyond the middle of the periodic system a-emission becomes


energetically possible for all nuclides along the band of fl-stability. Alpha
decay lifetimes are, however, strongly dependent upon a-decay energies, and
only when the decay energy exceeds a certain value do the lifetimes decrease
into the range where radioactivity can be detected. Since the potential bar-
rier against a-decay increases with atomic number, the "critical" a-decay
energy increases with atomic number. As a rough gauge of this effect we may
say that the energy required for a half life of 10TM years is 2 Mevin the region
of Sm(atomic number 62) and 4 Mev in the region of U (atomic number 92).
The energy dependence in the heavy element region is such that doubling the
energy (4 Mevto 8 Mev) decreases the half life by a factor of more than ~°.
The general energy trends along the line of maximum~-stability are indi-
cated in Figure 1 which is similar to a drawing published by Kohman(4).
The curve was constructed by making use of available mass data in the
region in which a-emission is not discernible. Aside from the smooth curve
showing a-decay energies, three other lines are shown. One of these simply
shows the line of demarcation between stability and instability toward
a-emission, and the other two show the approximate positions at which half
lives would be l0 s years and 10-4 years (~1 hr.). As mentioned, the smooth
curve goes through the center of fl-stability for each mass number. If we also
consider neutron deficient isotopes of each element, it will be found that
their a-decay energies are greater, a point which will be considered in more
detail presently. Twosuch series of isotopes (for Gd and U) are indicated
points and segments of curves crossing the main curve. The position of shell
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ALPHA RADIOACTIVITY 159


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¯ MASSNUMBER
FIO. 1. Alphadecay energy profile. Brokenline portion of curve indicates region
where direct a-decay measurementsare absent. Plotted points on segments of cross-
ing curves pertain to knowna-emitters of Gdand U. Half life guide lines indicate posi-
tions of applicable lifetimes as a function of massnumber.

closures at 82 protons and 126 neutrons is readily seen through its influence
on a-decay energy.
The mass data available are not nearly accurate enough to define the
curve of Figure 1 with the precision required to be useful as a guide for
a-decay properties. Uncertainties of several Mev are present in most of the
data while a fraction of a Mev is sufficient to change a lifetime from the
region of easy observation to that of extremely long periods. The curve is
consistent with known a-decay properties and can be altered in detail as
more precise data become available.
Summaryof alpha energies.--A compilation of all a-energies in the heavy
element region is given in Table I. 2 The data shown for each a-emitter repre-
sent what is considered to be the most reliable set. In general, only those
a-groups actually measured are included, although from 3’-ray and conver-
sion electron data there may be evidence for other a-groups. In a few cases
a-~ coincidence measurements showed the presence of a new a-group in
coincidence with a specific 7-ray, but the a-energy could be better defined
from that of the 3’-ray. Where the interpretation was unambiguous such

* Mostof the references for data shownhere and in Figure 2 will be found in the
1953Table of Isotopes (reference 25). For newerdata consult the following: ~°~ (5),
Em2n (6), 218 (7), Em~20(8), Ra ~r2 (7), Ra~* (9), Thm (7na (9), Th 2s° (10, 113),
Th*u (11), ~at (114), U~30 (7), Uu~ (8), U23~ (12), U~3~ (11), Pu28t (115), Pu~aa(13),
Pu~’° (8), =’’ (8), Pu~’~ (8), Am~’~ (14), Am=4~(14), Cm=4~(116), Cm =as (8, 15), CmTM
(16), ~a~(17), Cf ~4n(18), Cf ~ (19), Cf ~ (17, 19, 20), Cf ~° (17, 19, 20), Cf ~= (17,
19, 20), 992~r(21), ~a (19, 20, 22, 23), 10 -~ (19, 22, 23, 24) and 100=~ (19)
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160 PERLMAN AND ASARO


TABLE I
ALPHAPARTICLEENERGIESANDABUNDANCES

Alpha Alpha particle Relative abun- Type of


emitter energy (Mev) dances (%) measurement

Bi<1~8(1.7 m.) 6.2 ion ch


19s
Bi 5.83 ion ch
~9
Bi 5.47 ion ch
~°~
Bi 5.15 ion ch
~9~
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Bi 4.85 range
~°~
Bi --~3.15 range
Bim° (~10~ y) 4.93 ion ch
m
Bi 6.272 16 spect
6.618 84 spect
m
Bi 5.481 0.016 spect
5.603 1.1 spect
5.622 0.15 spect
5.765 1.7 spect
6.047 69.9 spect
6.086 27.2 spect
m
Bi 5.86 ion ch
m
Bi 5.444 55 spect
5,505 45 spect
~°°
Po 5.84 ion ch
~°~
Po 5.70 ion ch
~
Po ~.59 ion ch
~°~
Po 5.37 ion ch
~°~
Po 5.2 ion ch
~8
Po 5.064 4 spect
5.218 96 spect
~°~
Po 5.10 ion ch
*°s
Po 5.108 spect
~0~
Po 4.877 spect

Po 4.,~ weaL: a-3’ colnc.
5.299 100 spect
Po~n (0.52 s) 6.56 0,53 spect
6.88 0.50 spect
7.434 99 range
Po~’~?(25 s) 7.14 ion ch
~t~
Po 8. 776 spect
~’~
Po 8.336 ion ch
TM
Po 7.680 spect
*~
Po 7.365 range
~s
Po 6. 774 spect
~17
Po 6.5 ion ch
~
Po 5.998 spect
<~
At 6.50 ion ch
<~°~
At 6.35 ion ch
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ALPHA RADIOACTIVITY 161


TABLEI--Continued

Alpha Alphaparticle Relative abun- Type of


emitter energy (Mev) dances (%) measurement

~°~
At 6.10 ion ch
TM
At 5.90 ion ch
*°7
At 5.75 ion ch
At~°° (1.7 h) 5.65 ion ch
~°~
At 5.65 ion ch
~1°
At 5.355 37 spect
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5.437 31 spect
5.519 32 spect
m
At 5.862 spect
~u
At 9.2 range
*~4
At 8.78 ion ch
m
At 8.00 ion ch
~1~
At 7.79 ion ch
m
At 7.02 ion ch
~ls
At 6.63 ¯ range
m
At 6.27 ion ch
2°s
Em 6.138 spect
~°~
Em 6.02 ion ch
~1°
Em 6.036 spect
m
Em 5.605 ,~1.5 spect
5.778 67 spect
5.847 33 spect
m
Em 6.262 spect
~n
Em 8.6 ion ch
~16
Em 8.01 ion ch
m
Em 7.74 ion ch
~ls
Em 6.53 weak a-3’ colnc
7.127 100 spect
m
Em 6.214 4 spect
6.434 12 spect
6.559 15 spect
6.824 69 spect

Em 5.747 ~0.3 spect
6.282 100 spect
~
Em 5.486 spect
21.
Fr 6.339 24 spect
6.387 39 spect
6.409 37 spect
~1~
Fr 8.3 range
m
Fr 7.85 ion ch
.1~
Fr 7.30 ion ch
n0
Fr 6.69 ion ch
~
Fr 6.05 ~25 ion ch
6.30 ~75 ion ch
~u
Ra 6.90 ion ch
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162 PERLMAN AND ASARO

TABLEI--Continued

Alpha Alpha partide Relative abun- Type of


emitter energy (Me~) dances (%) measurement

*x9
Ra 8.0 ion ch
~0
Ra 7.43 ion ch
~’~
Ra 6.71 ion ch
~
Ra 6.23 weak a-3, coine
6.554 100 spect
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~
Ra 5.419 3 spect
5.487 2 spect
5.528 9 spect
5.596 24 spect
5.704 53 spect
5,730 9 spect
5.860 weak spect
~
Ra 5.445 5.2 spect
5.681 95 spect
~
Ra 4.592 5.7 spect
4,777 94 spect
Ae~ 7.6 range
~
Ac 6.96 ion ch
~
Ac 6.64 ion ch
m
A6 6.17 ion ch
~
Ac 5.80 ion ch
Ac~ 4.942 spect
~23
Th 7.55 ion ch
Thin 7.13 ion ch
Thm 6.57 ion ch
Thm 6,037 0.6 spect
6. 100 1.8 spect
6.228 21 spect
6.336 77 spect
~7
Th 5.651 ~-~2 spect
5.704 15 spect
5. 728 ,~1 spect
5. 749 17 spect
5. 796 2 spect
5.860 4 spect
5.922 ~2 spect
5.952 13 spect
5.972 21 spect
6.001 5 spect
6.030 19 spect
~9
Th 5.173 0.2 spect
5.208 0.4 spect
5.338 28 spect
5.421 71 spect
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ALPHA RADIOACTIVITY 163


TABLEI--Continued

Alpha Alpha particle Relative abun- Type of


emitter energy (Mev) dances (%) measurement

~9
Th 4.85 ~70 ion ch
4.94 ,~20 ion ch
5.02 ~10 ion ch
~o
Th 4.437 0. O7 spect
4.471 0.2 spect
4.613 23.4 spect
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4.682
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76,3 spect
*n
Th (3.93) 24 3" energy
3.994 76 ion ch
W
Pa 6.81 ion ch
m
Pa 6.46 ion ch
**s
Pa 5.85 25 ion ch
6.09 75 ion ch
n~
Pa 5.69 ion ch
z~t
Pa 4.660 1-3 spect
4.720 t1 spect
4.838 3 spect
4.938 25 spect
4.998 23 spect
5.015 23 spect
5.042 i1 spect
n~
U 6.8 ion ch
~
U 6.67 ion ch
n~
U 6.42 ion ch
~a°
U 5.662 0.8 spect
5.819 31 spect
5,888 68 spect
m
U 5.45 ion ch
m
U 5.132 0.3 spect
5.261 32 spect
5.318 68 spect
~
U 4.731 2 spect
4.780 15 spect
4.823 83 ion ch
~
U 4.59 --~0.3 a-3" coinc
4.714 26 spect
4.763 74 ion ch
~
U 4.20 4 ion ch
4.40 83 ion ch
4.47? ,~3 ion ch
4.58 10 ion ch
~
U (4.43) 27 3’ energy
4.499 73 ion ch
~9
U (4. 135) 23 3’ energy
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164 PERLMANAND ASARO


TABLE
I--Continued

Alpha Alphaparticle Relative abun- Type of


emitter energy (Mev) dances (%) measurement

4.182 77 ion ch
~3~
Np 6.28 ion ch
~
Np 5.53 ion ch
Npm 5.06 ion ch
~3~
Np 4.77 ion ch
~
Pu 6.58
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ion ch
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~
Pu (6.14) 14 3" energy
6.19 86 ion ch
pum 5.85 ion ch
*s~
Pu (5.71) 20 3’ energy
5.75 80 ion ch
~38
Pu 5.352 0.1 spect
5.452 28 spect
5.495 72 spect
~g
Pu 5.099 11 spect
5.137 20 spect
5.150 69 spect

Pu 5.014 0.1 spect
5.118 24 spect
5.162 76 spect
u~
Pu 4.848 25 spect
4.893 75 spect
~
Pu 4.854 20 spect
4.898 80 spect
~7
Am 6.01 ion ch
~g
Am 5.75 ion ch
m
Am 5.379 1.4 spect
5.433 13.6 spect
5.476 84 spect
5.503 0.2 spect
5.535 0.3 spect
~
Am 5.171 --~3 spect
5.225 13 spect
5.267 84 spect
~as
Cm 6.50 ion ch

Cm 6.25 ion ch
~a-
Cm 5.95 ion ch
vn
Cm 5.965 0.035 spect
6.066 26.3 spect
6.110 73.7 spect
~as
Cm 5.679 3 spect
5.732 13 spect
5.777 78 spect
5.985 6 spect
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ALPHA RADIOACTIVITY 165


TABLEI--Continued

Alpha Alphaparticle Relative abun- Type of


emitter energy (Mev) dances (%) measurement

~"
Cm 5.755 25 spect
5.798 75 spect
m
Cm 5.34 ~on ch
m
Bk 6.20 17 ~on ch
6.55 53 ion ch
6.72 30 ion ch
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m
Bk 5.90 34 1on ch
6.15 48 ion ch
6.33 18 ion ch
24.
Bk 5.4 ion ch
m
Cf 7.15 ion ch
~o
Cff 6.711 22 spect
6.753 78 spect
~4s
Cf 6.26 ion ch
~’
Cf 5.82 90 ion ch
6.00 10 ion ch
~0
Cf 6.0~ ion ch
a~
Cf 6.13 ion ch

~7
99 7.35 ion ch
~
99 6.62 ion ch
~4
100 7.20 ion ch
~5
100 7.1 ion ch

a-groups are included. Similarly, an a-group may be included which is not


directly observed because it cannot be resolved from a neighboring intense
group, but for which 3,-rays or conversion electrons define this group un-
ambiguously. Such a-energies are enclosed in parentheses and the type of
measurement designated as ’"y energy." We have arbitrarily omitted the so-
called "long range a-partlcles" of Pom and Po~u (even though they do ap-
pear in low abundance in the spectra) since these are not transitions from the
ground states or from measurable metastable states.
It is difficult to assign meaningful limits of error for the individual meas-
urements and they are omitted. In general, those made with a spectrograph
may be in error by as much as 15 key, but a large number are perhaps ac-
curate to less than 5 kev; those made by the ionization chamber method will
vary in accuracy from 10 to 75 key; and range measurements in photographic
emulsions are even more difficult to assess. Energy differences between
groups in a particular spectrum are in general more accurate than the abso-
lute a-energy. Most energies determined are not absolute but depend upon
comparison with standards, so a list of some of the most accurate values
(absolute and comparative) suitable for standards are shown in Table II.
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166 PERLMAN AND ASARO


TABLE II
ABSOLOTE
ALPHAPARTICLEENERGY
DETERMINATIONSINCLUDING
SOMEVALUES
MEASURED
RELATIVETO RaC’*

iSturm Rosen- Collins, Best


Lewis, MeKenzie,
Alpha Briggs and blum, value,
Bowden
emitter (3) Johnson Dupouy and Briggs
(29)
(27) (28) Ramm(30) (26)

RaC’ 7.680 7.683 7.680


~1~)
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(Po
ThC’ 8.776t 8.780 8.776t 8. 786 8. 780
m)
(Po
~t0
Po 5.298 5.299 5.299 5.305 5.301
t
ThC 6.082t 6.087 6.082~ 6.090 6.086
(Bim)a0
ThC 6.043~ 6.048 6.042~ 6.050 6.047

* All measurementscited were madewith magnetic spectrographs except those of


Sturm & Johnson (27) whoused an electrostatic device. The values listed for the
magnetic measurementswere corrected as done by Briggs (26) in terms of slight re-
visions of fundamentalconstants used in the conversion of Ha to energy.
’f Measuredrelative to RaC’.

Alpha decay energy systematics.--The value of a curve such as that in


Figure 1 is to help visualize in broad outline the conditions and regions of
a-instability. A good deal more is to be learned from a more detailed exami-
nation of the regions where a-radloactivity is prominent. It is observed that
a-decay energies ~ fall into well behaved patterns, the recognition of which
has proved considerably useful for a number of purposes. Two of the func-
tions of these correlations will be mentioned.
Alpha decay series (containing relatively f~w/~-decay steps) provide
continuous series of energy increments from the region of the element Pb
to the highest elements possible. The many decay chains either combine
through decay or can be related energetically by measured neutron binding
energies. By analyzing these data, it is possible to obtain a rather detailed
picture of the energy surface 4 in the heavy element region. The shape of the
~ Alpha decay energy or simply decay energy will refer to the Q value for the a-
emissionprocess and is therefore immediatelytransferable into a massof energy differ-
ence between ground states of parent and daughter. The actual a-particle measured
for the ground state transition is of appreciably lower energy because of the energy
carried off by the recoil atom. Of course, the a-groups leading to excited states are
of still lower energy. The measuredenergies of a-groups will be referred to as
particle energies" or "particle energies" to distinguish them from "decay energies."
4 "Energysurface" refers to a surface defined by the energy contents or masses of
the nuclides.
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ALPHA RADIOACTIVITY 167


energy surface is readily delineated from these data, and regions of greater
ot lesser stability stand out clearly. A schematic representation of such a
surface, exaggerated for purposes of illustration, was given by Perlman,
Ghlorso & Seaborg (31). A complete and critical compilation of all decay
energy data, and the atomic masses calculated from these has been made by
Seaborg & Glass (32). The data include masses of nuclides not yet prepared
and these were derived from decay energies estimated by methods which
will be indicated below.
Of great value to the experimentalist has been the ability to predict a-en-
ergies, and the agreement between predicted and measured values often serves
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IO.C

!\ ",Fr

, ’~ ,,, ~, ,,

4.(

204 2t2 220


MASS NUMBER

Fro. 2. Alpha decay energy versus mass number.

as a criterion for isotopic assignment. Furthermore, if the energy can be pre-


dicted, the half life can be calculated. The forecasting of both a-energy and
half life has been of inestimable value in the preparation and identification
of higher and higher elements.
A number of systems for correlating a-decay energies have been employed
and perhaps that most widely used is illustrated in Figure 2. Here, the iso-
topes of each element on a mass number versus energy plot are joined, re-
sulting in a family of curves which over a wide region comprise a series of
nearly parallel lines. It will be noted that in this region (above mass number
~212) a-energies decrease with increasing mass number for each element;
that is, with increasing neutron number. This system in some modification
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168 PERLMAN AND ASARO


has been used by a number of workers (31, 33 to 37), while others have used
contour map presentation (38, 39) and still different methods (40).
Before turning to the regions in Figure 2 where sharp changes in the lines
occur, let us consider the broad region of regular behavior. The semi-empiri-
cal method of calculating atomic masses of Weizs~cker (41), as developed
further by Bethe & Bacher (42) and by Bohr & Wheeler (43), pictures
energy surface as a trough having parabolic sections at constant mass num-
ber, A. The bottom of the trough goes through the fl-stable nuclides and if
the energy coordinate is expressed in terms of the mass defect, the llne along
the bottom becomes the familiar "best" mass defect curve. It can be shown
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graphically (31) or analytically (4) that the observed trend of a-energy


mass number (Fig. 2) is to be expected from this picture. Differences in slope
and spacing of the lines can be interpreted in terms of departures from ex-
treme regularity of the trough such as small changes in curvature of the
trough or of its slope.
The dramatic inversion in the a-energy trend around mass number 212
is a consequence of the major closed shells in this region (37, 44). Wecan see
what happens more precisely by following the curve for the Po isotopes.
From Po~18 down to Pom the curve follows the normal trend; then Pom is
seen to have considerably lower a-energy than Po21~. This can readily be
shown to be a reflection of the fact that the binding energy of the 126th
neutron in Pb (Pb~07-PbI°8) is greater than that of the 128th neutron in Po
(Pom-Pom). Similarly, since the binding energy of the 125th neutron in
(pb~06-pb~°7) is greater than that of the 127th neutron in Po (Po~0-po~n),
the a-energy of Po~l° is lower than that of Pom. After the neutron shell of
126 is well passed and the neutron binding energies change monotonically
for both parents and daughters, the regular trend of increasing a-energy with
decreasing neutron number is resumed (see region between Po~°8 and Po~83).
The curve for Bi is seen to parallel the Po curve with a wide energy spac-
ing between them. This energy spacing is presumably a consequence of the
82 proton shell. The reappearance of a-radioactivity in highly neutron de-
ficient isotopes of Bi (45) was the clue needed to establish the generalness
this effect of crossing the region of 126 neutrons (44 to 52).
It will be noted that the a-energies for the isotopes with 128 neutrons
would be expected to become progressively greater for each higher proton
number. Half lives will accordingly be very short in this region so that
preparation and identification of such nuclides would be difficult. However,
more neutron deficient isotopes should be more stable just as Po.1° is more
stable than Pom. Such a region has been found for At, Era, and even for Ra,
showing that the effect of 126 neutrons extends at least this high (51, 52).
Undoubtedly these points shown on Figure 2 join to those of higher neutron
number by going through sharp peaks higher than those shown for Po and
At.
The question arises as to whether or not there is evidence for other closed
shells or subshells on the basis of a-decay data. A situation similar to that
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ALPHA RADIOACTIVITY 169


at 126 neutrons, but considerably more subdued, seems to occur at neutron
number152 (19). The evidence comes principally from the a-energy trend
of Cf isotopes (element 98) as seen in Figure 2 showingthat the Cf isotope
with 154 neutrons has a higher energy than those of the next few isotopes of
lower mass number. The fragmentary data on elements 99 and 100 are not
out of llne with this concept and the lines are drawnin Figure 2 according
to expectations. As will be explained later, the positions of closed shells can
be correlated with energy level spacings betweencertain excited states and
their ground states but, in this respect, the single nuclide knownwith 152
neutrons (Cm24s from a-decay of CP~) does not reflect a closed shell con-
figuration (53, 54).
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It will be noted in Figure 2 that the energy increments from isotope to


isotope along manyof the curves are not very uniform. Aside from the marked
inversion ia trend in the region of Pb and the probablesmall inversion in con-

~ 237
241
~m 245
0233
0.02
241
~----.--
~- 90+h233
4.~.~-
¯ 921 5.13
u ~
5.72

FIo. 3. Decaycycles for part of 4n+l family. Code:~-a-decay,T negative #-


decay, ~ electron capture decay. Numeralsindicate energies in Mev;those with
superscript"c" are calculated by dosingthe cycles; those with superscript "~" are
estimatedas by the use of Figure2; those unmarkedare measured values.

junction with 152 neutrons, it is seen that in someplaces the isotopes seem
bunchedand in others relatively spread out. It has been suggested that there
are subshells at 92 protons (55, 56) and at 88 protons (56) in explanation
someof these irregularities. Other inferences of a-decayenergies on possible
subshells have been discussed by Broneiwski(57).
Decay energies from energy-balance cycles.--As a guide in research on
newheavyisotopes, the ability to predict decayproperties is of great value.
By interpolation and extrapolation, the curves of Figure 2 maybe used to
estimate a-energies and these as well as measuredvalues can be used in con-
structing a self-consistent systemof energy-balancecycles whichcan be used
in turn to calculate degrees of ~- instability and other a-energies.
To illustrate this methodof correlating decay energies (32), a segment
of the decay cycle representation of 4n-]-i types nuclei is shownin Figure 3.
A few examplesof the uses of these cycles will be mentioned.It is noted that
by makinguse of three measureddecay energies the a-energy of the 6.8 day
n Thetype "4n q-1" meansthat all massnumbersare divisible by 4 with remainder
1. All nuclei connectedby a- and #-decayprocessesare of the sametype.
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170 PERLMANAND ASARO


~37
¢t- emitter U is calculated to be 4.25 Mev.This is almost identical with
the decay energy of U~8 whichhas a half life of 4.5 X109years. The partial
a-decay half life of U~37 wouldbe expected to be at least as long. Accord-
ingly, the a-branchingof U~3r wouldbe only of the order of 10-13 so that this
modeof decay wouldbe most difficult to observe. On the contrary, the a-
branching of Pu~4t was similarly estimated to be about 10-~ whichwas within
reach for measurementand the o~-energy as subsequently measuredis shown
in Figure 3.
Anotheruse of these cycles has to do with predictions of 0-stability. If
one considers the possibility that am~45 is a if--emitter and that its prepara-
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tion wouldtherefore also produce Bk~4~, the idea should be rejected because
it is seen that Bk~45 is unstable with respect to Cm ~4~by about 0.7 Mev.The
~
estimated a-energy of Cm which goes into this calculation cannot possibly
be in error by an amountto reverse this conclusion.
An extension of these cycles to still higher elements gives a meansof
making predictions into a region where measurementshave not been made,
and these predictions serve as an important guide to the experiments. Other
cycles can be devised to join different nuclear types through measuredbind-
ing energies. With a single neutron binding energy measurementjoining two
series, other neutron binding energies can be calculated (32).
Alpha emitters just below tead.~The removal of neutrons from any ele-
ment increases the potential toward a-decay and this is the basis for the
main trend in Figure 2. Alpha active nuclides of Au and Hg have been pre-
pared by removingmanyneutrons from the stable isotopes (58). In the ease
of Au, the stable isotope Au~97 is estimated to have an a-decay energy of
only 1 to 2 Mev,while the isotope observed with an a-energy of 5.1 Mevis
believed to lie in the massnumberrange 183 to 187. As neutrons are removed,
successive isotopes becomemore unstable toward orbital electron capture
also, but since a-decay lifetimes are extremelysensitive to energy, this mode
of decay should at somepoint becomediscernible.
One other a-emitter in this region has been reported (59), a component
of natural W.The extremely low specific activity seemsout of line with the
measured energy (3.2 Mev) if the emitter has the abundance of one of the
knownWisotopes, so the authors postulate the existence of a rare isotope
(Wxrs) in the natural mixture in amountstoo small to detect by mass spec-
troscopy.
Rare earth alpha emitters.~Amongthe rare earth elements we pass through
a region where stable or slightly deficient nuclides can decay by a-emission
~4n
to the dosed shell of 82 neutrons, Such a nuclide with 84 neutrons is Sm
whichis 0-stable but missing in nature because of its relatively short a~half
life (~5×10r years) (60). The a-energies are summarizedin Figure 4
although the curves are fragmentary as compared with those in the heavy
element region, the basic structure as related to the 82 neutron shell is un-
mistakable. The point assigned to NdTM TM is of special interest because Nd
is a componentof natural Nd (61).
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ALPHA RADIOACTIVITY 171

Tbl~’ ~(?)
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2.¢

I I
1.50 160
MASS NUMBER
FIG. 4. Alpha decay energy versus mass numberin the rare earth region.

COMPLEXALPHASPECTRA
As in other decay processes, the appearance of multiple groups in the
a-emission process may be considered as the result of competition in populat-
ing available energy levels. It will be seen that a-decay lifetimes are in-
fluenced by a number of factors and among these is the sharp dependence of
lifetime with decay energy. Consequently, it would not be expected that
transitions to high-lying levels (say 1 Mev) would be readily observed.
There are, however, selection processes operating which can delay the highest
energy group and cause lower energy groups to be the most prominent. As
yet, there is no systematic formulation of "selection rules" for the a-decay
process. The development of a-decay theory with this as an objective is
undoubtedly the most important step now faced.
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172 PERLMAN AND ASARO


The present discussion will be concerned largely with the regularities
which are appearing with respect to the location of energy levels, their
spectroscopic designation, and in the degree to which these states are popu-
lated. As already stated, only a start has been madein developing reasons
for preference in populating certain states.

EVEN-EVE~ALPHAEMITTERS
Principal alpha groups(the groundstate and first excited state).--With
high degree of certainty it can be said that the transition to the groundstate
is the most abundant for this nuclear type. In each of the manycases which
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have been examinedin detail, the main a-group is that of highest energy and
there is no evidencethat the groupis followed by "/-radiation. To this extent
at least the even-even a-emltters are well behaved according to existing
a-decay theory.
In examining a number of even-even a-emitters around U and in the
transuranium region, it was noted that each had a second prominent a-group
of some40 to 50 kev lower energy than the ground state transition (62). The
abundance of this group was always in the range 15 to 30 per cent. 8 (We
shall see presently that the states reached by these a-groups apparently all
have spin 2 and even parity and we shall call each the "first even spin
state" or simply the "first even state.") ~ Whenlower elements or lower
neutron numbersof a particular element are considered, the same states are
identified but the energy level spacings above the ground states become
progressively greater and the abundances of the a-groups populating these
states progressively lower. A summaryof the energy spacings between the
ground state and first even state as a function of neutron numberand proton
numberis shownin Figure 5. The points divide into families according to
atomic number and appear to reach maximafor nuclei with 126 neutrons.
In somecases, the points in Figure 5 were determined from "/-ray spectra
rather than from observation of the a-groups.
It has already been deduced by several authors (63, 64, 65) that the
first excited states of even-even nuclei in general are 2+ states and this
applies to regions other than that of the heavy elements and irrespective of
the particular energyspacing of the levels. There is theoretical justification
for the 2+ assignment both from modifications of the independent particle
model(66, 67) and from the collective model(68, 69). There is also theoreti-
cal explanation (67, 69) and empirical proof (62, 65, 70, 71) that the energy

6 Weshall define "abundance" to indicate the number


of a-particles in a particular
grouprelative to the total numberof a-particles.
~ It is worthrecalling that in conservingparity in the a-decayof an even-even
emitter, the evenspin states musthaveevenparity and the oddspin states oddparity.
A corollaryis that -r-ray transitions fromany of these excited states to the ground
state mustbe electric transitions andnot magnetic.
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ALPHA RADIOACTIVITY 173


IOg

¯ ALPHAENERGYDATA
x GAMMADATA
X
I

I
I
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I
I X
I,¢

,
Pb ~
×

0.I

,.- ! I , I

NEUTRON NUMBER
FIG.5. First excitedstate energiesof even-even
nuclei in the heavyelementregion.

level spacing for the first excited state goes through a maximum at each
closed shell as is seen in Figure 5 for the 126 neutron shell.
Twotypical even-even a-spectra are shownin Figure 6 and for the pres-
ent we shall focus attention on the two lowest states corresponding to the
two a-groups considered. The states assigned 2 + are the "first even states"
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114 PERLMAN AND ASARO

228
Th 242
Cm

....//I
/ 0.035%/

//.
73.7

305 i f, 6+

/
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O+ 0
224 2~8
pu
Re
~h’~IG- 6- Decayschemes of Th~s ~.
and Cm

already mentioned and are designated so because they de-excite to the


ground state by electric quadrupole (E2) transitions. 8 Since there is no evi-
dence to the contrary, we shall assume that the "first even state" is in each
case the "first excited state."
Rare alpha groups (higher even states and first odd state).--Many of the
a-emltters which have lent themselves to detailed analysis have proved to
have one or more additional groups of lower energy and in low intensity.
The low intensities of these groups are not attributable alone to lower energy
than the two main groups. If we calculate the lifetimes for the ground state
transition and that to the first excited state according to current a-decay
theory, the results are in substantial agreement with the measured lifetimes.
However, the measured partial half lives for the higher transitions are con-
siderably longer than the calculated values and we refer to such transitions
as "hindered." This subject will be dealt with under the section on a-decay
theory, and for the present we will consider only the energy level spacings
and spectroscopic assignments.
In each case which could be examined in the necessary detail, there was
s The nature of the transition has been deduced from measurementsof absolute
conversion coefficients, relative L subshell conversion coefficients and a-~, angular
correlations. The cases studied are the a-emitters Po~° (72), =~ (7), Ra ~4 (73, 74
75), RaTM (75), TM (7), Th~8 (9, 76, 77, 78), Th~° (77, 79), U~a6 (7), U~a (8), U~(8)
U~ (80), ~s (13), Cm~ (1~), an d Cf~ (89). Th e ex cited st ates in question bel ong,
of course, to the a-decay products:
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ALPHA RADIOACTIVITY 175


found a rare a-group going to a state which decays by an E2 transition only
to the 2+ state. 9 These states are those designated as 4+ in Figure 6 and
will be known as the "second even states." From the nature of the 3"-ray
transition, the second state could be 0+, 2+ or 4+; the 4+ assignment is
made largely from a theory to be mentioned presently which fixes it as a
member of a rotational band of states 0+, 2+, 4+ ¯ ¯ ¯ . The fact that no
crossover transition is seen from the second even state to the ground state
may also be taken as partial evidence for the assignment.
In a few cases, very rare "),-rays have been seen (the a-groups would
below the limits for detection) and are assigned to transitions between the
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third and second even states (13, 15). In the case of ~s decay (1 3), th
3,-ray was shown to be in coincidence with that between the 4+ and 2+
states. Since the energy of the state defined by the 3,-ray corresponds closely
with expectations if it were the third "even state" (6+) of the rotational
band, it has been so designated (see Cm ~4~ spectrum, Fig. 6). The theory be-
hind these assignments will now be examined.
According to a theory of Bohr and Mottelson (68, 82), collective aspects
of nuclear motion and individual particle aspects are coupled. In a "region
well removed from a closed shell" there should be a series of energy levels
corresponding to a rotational band in which only even states (0+, 2+,
4+ ¯ ¯ ¯ ) appear for an even-even nucleus. On this basis, electric quadrupole
transitions should predominate. Another requirement of the rotational spec-
trum in this region is that the states lie at energies proportional to Ii(Ii+1),
where I i is the spin of the jth even state. For the levels 0+, 2+, 4+, 6+,
the ratios of 4+/2+ and 6+/2+ would therefore be respectively 3.3 and
7.0. Figure 7 shows an extensive set of these ratios of the first and second
even states, and it is seen that the agreement with expectations is excellent
for the higher neutron numbers but gradually departs as the region of 126
neutrons is approached. Apparently the same behavior can be noted for
even-even nuclei in the rare earth region in reference to the 82 neutron shell
(83). The point for ~s inFigure 7 i s of questionable sig nificance sin ce it is
~°~
not at all certain that the first two excited states as deduced from T1
fl--decay are indeed 2+ and 4+. As an example of this uncertainty, a num-
ber of different measurementsconcerning the first excited state have resulted
in different assignments: 1+ or 2+ (84), 2+ (85, 86, 87), 3- (88).
cases, Pu2~8 and UTM, (a-decay of Cmmand Pu2~) where a third even state is
inferred, the energy ratio of this level to the 2+ level is indeed close to 7.0.
The evidence for the higher state in the case of Pu~38 decay is that the 3,-ray
used to define it is in coincidence with the 3,-ray from the 4+ to the 2+
states (13).

0 Conversioncoefficient data defining the transition as E2 have been obtained in


~ (15) ~a8 (13, 81), U~a2 (8), Th 2~s (9). For ot her cases there is
the a-decay of Cm
direct information, but other regularities to be discussed presently makeit highly
likely that comparablestates are being considered.
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PERLMAN AND ASARO

x FROM GAMMA RAY DATA


¯ FROM ALPHA PARTICLE DATA
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..J 4
.r~,226 ~,_228 Th230 UTMU_~36 24z
Crn
>- - ~ ~= Y,---- @-----|__ =-X. ......
L¢3~ 23~
PU
uJ 3 Th
z

I pb208

I I I I I I I I I I I I
0
126 130 134 138 147 146
NEUTRON NUMBER
FIG. 7. Ratios of energiesof the secondand third evenspin state to the first ex-
cited state. Thebrokenlines represent the expectedvalues fromthe Bohr-Mottelson
theoryfor rotational levels in regionsremoved
fromclosedshells.
In a numberof cases, a state believed to be 1- has entered amongthe
low-lying even states. The spectrum for Th=s which is typical of this type is
shownin Figure 6 (9). In contrast to the secondeven state, this state always
decays both to the first even state and to the ground state. The conversion
coefficients of both conformwith E1 transitions (9) as do more recent a-~/
angular correlations made on Th~, Th~a and U~a° (89).
The 1 - state has probably been identified in the decay of Th~° ~n and U
as well as for the three cases just mentioned.Significantly this state has been
identified only amongthe low-lying excited states of nuclei of neutron num-
bers in the range 134 to 138 neutrons. From the fragmentary evidence at
hand it seems possible that the state has a minimum energy at 136 neutrons
and rises at both lower and higher neutron numbers.
With respect to the degree of population of the 1 - state in the a-decay
process, the data are too few to arrive at any generalizations. In the cases
studied, the process seems to be competitive with that leading to the 4-t-
state for comparableenergies.
Finally, it should be remarkedthat there is no ready explanation for a
low-lying odd parity state such as this. Neither the independent particle
modelnor the collective model wouldpredict such states in any straight-
forward manner.
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ALPHA RADIOACTIVITY 177


ODD NUCLEONALPHAEMITTERS
The a-spectra of nuclei having odd nucleons are in general considerably
more complex than those of even-even nuclei and consequently have not
been worked out with the same degree of certainty. Also, they may differ
from each other considerably and have not yet yielded to a comprehensive
generalized picture such as applies to the even-even nuclei.
Nevertheless, some regularities can be discerned, and amongthese is the
appearance of rotational bands (14, 90) closely similar to those of the even-
even nuclei. Interestingly enough, the fundamental state of the rotational
band (where such a band shows up distinctly) is that populated in highest
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abundance, but it need not be the ground state and perhaps usually is not.
The important implication of such spectra with respect to a-decay theory is
that powerful "selection rules" are in force since the highest energy transi-
tion (that to the ground state) is often in very low intensity (91).

233
U 4~
Am2. AmZ43 Cm~4;~

98.8+6 97+ 102+27

Np
Np~59.

0~ I/~
239
pu

FIG. 8. De~yschemes
of someodd-nucleon~-emitters.

Figure 8 showssomespectra which were selected to illustrate someoE the


regularities noted.TM (Obviously [t is not possible to discuss all spectra of
these types and some,such as that for Th~; with eleven reported groups (92),
are too complexfor analysis at present.)
The partial spectrumfor U=~ is not representative of most of those ex-
amined Jn that it looks much like that o~ an even-even a-emltter. The
energylevel spacings for these states are muchlike those of Cm ~ (see Fig. 6)
and the relative populations of the states are roughly comparable, but an
important difference to be noted is that the secondexcited state decaysboth
to the ~rst exc[ted state and d{rectly to the groundstate. ~ possible exp]a~a-
~ (14, 91) ~*~
~ Thereferencesfor the data comprisingthese a-spectra are Am
(14), u~ *"
(8, 15), U (8).
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178 PERLMAN AND ASARO


tion of this spectrum lies in its interpretation as a rotational band, the
grounds for which are now sketched.
According to Bohr & Mottelson (68), the rotational band for a nucleus
with an odd nucleon will have a fundamental state of spin I0 and higher
states of spins Io+l, 10+2, ¯ ¯ ¯ , all with the same parity. The spacings of
these levels will go as W+CI(I+I), where W and C are constants for a
particular level sequence. For the U2a3 case the following equations may be
set up:
E~8.o- E4~.~= C(Io + 2)(lo + 3) C(Io + 1)(Io + 2)56.1
2C(Io + 2) = 56.1
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F~,2.8 - Eo = C(Zo + 1)(10 + 2) Clo(1o + 1)= 42.


2c(I0 + I) -- 42.8.
The solution of the simultaneous equations gives I0--2.2 and since the spin
must be half integral we take the closest value, I0=5/2. It should be men-
tioned that this analysis is extremely sensitive to the accuracy of the data;
an error of only 0.5 key in the 42.8 kev level, making it 43.3 kev, would
change the calculated value of Io to exactly 2.5. if we accept 5/2 for the
fundamental state, the spins of the other two levels become 7/2 and 9/2.
The cascading ~/-ray transitions could then be M1 and/or E2 and the cross
over transition E2, which assignments are not out of order with the fact that
both crossover and cascade q,-rays are observed.
The spectra for Am2~1, Am~, and Cm~.3 a-decay show quite similar ro-
tational bands with calculated fundamental state spins of 5/2, but the
fundamental states in these cases are not the ground states. Americium 241
and Am~4~ differ only in that this state is respectively 60 and 75 kev above
the ground state. For Cm =43, the ground state transition has not yet bee~
observed even though it has 277 key higher decay energy than the main
group, a fact established by a-~’ coincidence counting (15).
It is perhaps not profitable at present to speculate in detail on the mean-
ing of the_complex spectra of the nuclear types under discussion. Webelieve
that rotational bands which can be explained as a consequence of collective
modes of nuclear motion are discernible. It is also probable that other im-
portant features of the spectra must bring in the concept of single particle
states. Just what these states are and what guides the a-decay process to
some and not others is still obscure. Some speculations on these matters as
they apply to a-decay theory will be brought out in the section on this sub-
ject. It is worth reiterating here that no simple criterion or rule is likely to
explain the spectra shown in Figure 8 as well as the extremely complex
spectrum of Th~=7 and that of Pu=~° which is a good deal simpler but different
from both types.

ALPHA DECAY LIFETIMES AND THEORY


It is possible to correlate a-decay lifetimes empirically and to arrive at
systems which can be used to predict half lives. For example, regularities can
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ALPHA RADIOACTIVITY
be observed in plotting the half life with the mass number for successive
elements. However, it is also possible to systematize the half lives in terms
of parameters which are involved in current a-decay theory and thereby also
obtain some information on the status of the theory.
It will be seen that the ground state transitions of even-even a-emltters
are treated with extraordinary precision by basic one-body a-decay theory.
However, analysis of the many a-spectra obtained during the past few years
has shown clearly that more elaborate theory is required to account for the
behavior of other nuclear types as well as for certain of the transitions to
excited states of the even-even nuclei. The development of new approaches
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to cover these cases is currently in a formative stage. It will not be possible


in this review to cover in detail either the old theory or the new approaches;
rather, we shall emphasize those aspects of a-spectra which appear to require
new forms for expression and indicate the direction some of these new forms
are taking.
Basis for one body theory.--The initial conception by Gamow(1) and
Condon & Gurney (2) of the a-decay process as a barrier penetration prob-
lem has been cast into a number of forms differing in detail but basically all
ending up with the decay rate expressed as the product of two factors: (a)
"frequency factor" which may be considered as the decay rate without the
barrier; and (b) a "penetration factor" which expresses the probability
an a-particle emerging through the negative energy region of the coulombic
potential barrier. The various solutions to the problem differ in the degree
of rigor which is applied, and it might be stated that the sensitive portion is
the "penetration factor" which is exponential in form and is handled virtu-
ally identically in the several treatments. (See, for example, references 93 to
97.)
The parameters which enter into the penetration factor are those which
define the barrier for the a-particle of energy E and these are the nuclear
charge and the effective nuclear radius. The frequency factor, likewise, is a
function of the energy of the a-particle and nuclear ~adius and although ap-
proximations are introduced in its evaluation, this factor is relatively in-
sensitive and does not strongly influence the results. It is probably here, how-
ever that the one body model breaks down as a representation of decay
processes, that is, where single particle states are of importance.
It will be noted that of these parameters the nuclear charge has explicit
meaning dissociated from the a-decay process and the a-energy and decay
constant are subject to precise measurement, but the effective nuclear radius
is a quantity which is not obviously meaningful for this process when deter-
mined from other nuclear phenomena, nor do such independent methods of
measuring the radius give the desired precision for testing a-decay theory.
The procedure to test the theory is therefore confined at present to see if
calculated nuclear radii fall into a reasonable range and pattern of values or
fluctuate in an unreasonable fashion (58, 93 to 100). Conversely, one may
assume some function for nuclear radii, from this derive theoretical curves
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180 PERLMANAND ASARO


to express the decay constant in terms of the other parameters, and test the
agreement with the measured decay constants (31, 98, 99, 101, 102). It
this second approach which has proved most useful in correlating a large
numberof data. Further discussion of this matter will follow as the data for
even-even a-emitters are examined.

U
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Pu
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Ern

Po


EFFECTIVETOTAL DECAY ENERGY (MEV)

FIG.9. Experimental valuesof log half life versusa-energy.("Effectivea-energy"in-


cludes correction of particle energyfor recoil and electron screenlng--seetext.)
Even-evenalpha emitters: groundstate transitions.--Figure 9 showsa plot
oI the half life versus energy relationship as a family of curves. The curves
are defined by the experimentalhalf lives and are in this respect empirical.
If, however,we were to calculate half lives with the Kaplan(99) modification
of the Preston (95) formula, by using the measureda-energy for each point
and assuminga function for the nuclear radius, 1.52 X 10-13 A1[3, the resulting
curves wouldlie close to those of Figure 9. In detail, the calculated curves of
the lower elements (Po, Era) would lie somewhatbelow the corresponding
curves of Figure 9 and for tile higher elements (Cm, Cf) the calculated
curves would lie slightly above those shownin Figure 9. (The segments of
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ALPHA RADIOACTIVITY 181

curves shown for Po*t° and Po208 and for Em~t° and Em208 should be con-
sidered as special cases in which effective nuclear radii suffer a discontinuity
and these are nuclei with 126 neutrons and fewer.) To bring about more exact
agreement one can bring in a second order effect by assuming that the nu-
clear radius parameter should not be a constant, 1.52, but should vary in
some fashion, say with atomic number. To see what is required, a calculation
was made for the effective radius of each nucleus using measured values of
both energy and half life and the results are shown in Figure 10. The sharp

1.60
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L58 ~ Em

u. L54

co 1.52
n
1.50

L44

I I 1 I I I I t I I
I~0 1~4 1~8 132 156 140 144 148 152 156
NEUTRON NUMBEROF PARENTALPHA EMITTER
FI6, 10, Nuclearradius parameter.

break at 126 neutrons is apparent but, in addition, there seems to be general


decrease in radius parameter with increase in atomic number. This, of course,
is a restatement of the relation mentioned between the empirical curves and
those calculated on the basis of a single average value for the radius param-
eter. With reference to the data of Figure 10, it should be pointed out that
there is sufficient experimental uncertainty in some of the values which went
into these calculations to shift the points by 0.02 unit of radius p~rameter
or even more.
In summary, we can say that the basic one body theory of a-decay ap-
plied to the ground state transitions of even-even a-emitters gives a remark-
ably consistent picture. By using reasonable and consistent assumptions for
the values of fhe nuclear radii, the theory explains observed half lives which
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i82 PERLMANAND ASARO


differ by a factor of 10~4. It should be pointed out that different formulations
of the theory will give somewhatdifferent "best values" for the radius
parameter, but each is internally consistent.
Twofurther points should be mentionedwlt, h respect t~ the curves of
Figure 9. It maybe noted that the energy values listed are somewhathigher
than measured particle energies. The a-energy pertinent to a-decay theory
is based on its center of massvelocity and therefore the particle energy must
be increased by the energy of the recoil nucleus. This correction amountsto
~100 kev for a 6 Meva-particle in this region.
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Anadditive correction to the a-particle energy so far overlookedhas been


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suggested by Ambroslno&Piafier (103) and has to do with the lowering


the potential barrier by the electron cloud. As discussed by Rasmussen(104)
this correction should be applied as an added a-energy amountingto about
the difference of total electron binding energies betweenparent and daughter
in the particular a-decay process. This amountsto ,-~38 key in the region of
U and is smaller for lighter elements. This latter "screening correction" to
the particle energies does not have a profound effect on the agreement of
theory and experimentwhich is under discussion, but it does have the effect
of giving somewhatsmaller values of nuclear radii than if it were ignored.
The other item concerning Figure 9 has to do with the reason that smooth
curves can be drawnat all because, in principle, each curve is not continuous
if the nuclear radius is an independentvariable. However,as seen in Figure 2,
a-energies vary more or less monotonically with mass number A and since
nuclear radii do so likewise, each value of energy (for a particular element)
does localize the mass numberand therefore the radius. Wheretwo isotopes
within the sameenergy range do have large differences in effective radii they
do not lie on the samecurve. This effect is seen for Po and Emcurves on the
two sides of 126 neutrons.
Even-evenalphaemitters: transitions to excited states.--For any particular
groundstate transition, one can calculate the partial half life to any excited
state under the assumptionthat the only factor influencing the relative de-
cay rates is the energyfunction. Let us first consider transitions to the first
excited state (2 q-). The effective radius as determinedfrom the groundstate
transition process is adopted and it is assumedthat the spin change, whether
zk/’=0 or AI=2, will not affect the decay rates very much. This latter as-
sumptionhas the theoretical justification of the calculations of Preston (95,
96) which show that contrary to previous treatments, a AI=2 transition
should be some1.5 times faster than a AI-~0 transition and that only when
AI=4 does the function take the direction of delaying the transition.
The ratios of expected abundances(solely from energy difference) to ex-
perimental abundances are shown in Table III. Around Ra, Th, and U the
ratios are seen to be close to unity and perhaps to rise significantly for the
heavier elements. Somerecent ideas on the population of these states will be
mentionedbelow wheretransitions to the 4-1- state are discussed.
One apparent anomaly is Po~°8, for which no a-group has yet been seen
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ALPHA RADIOACTIVITY 183


TABLE III
OF FIRST EVENSTATI~(2+) BY ALPHADI~¢A¥OF EVEN-EvEN
POFULATION NVCLEI

Energy Energy Departure


Alpha Departure Alpha
level level
emitter factort emitter (key)* factort
(key)*

*°~
Po 163 3.1 *~
U 52 1.2
*08
Po 374 >32 U*a6:~ 50 1.1
Po**°~ 800 1.6 U’68:~ 45 1. $
TM
Ra 240 I. 2 Pu~:~ 45 3. $
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m*
Ra 188 0.9 Pu~ 47 2.2
~
Th 110 1.2 ~3s
Pu 43 1.6
~8
Th 84 0.9 ~0
Pu 44 I. 7
~80
Th 68 1.0 Pu~ 45 2.2
Thl~:~ 65 0.8 ~**
Cm 44 1.7

U 70 1.1 ~**
Cm 43 1.8
*~
U 58 1.1 ~
Cf 42 2.7

* Energylevel of the 2-k state of the daughter nucleus.


~ Ratio of calculated abundance(solely from energy difference) to experimental
abundance.A factor of unity meansthat the l~fetime for the decayto this state (in this
case 2 +) is according to expectations from a-decay theory using the ground state
transition to define the nuclear radius and neglectlng any effect of spin change.
:~ The experimental abundancesor energies maybe suspect.

leading to the 374 kev 2 q- state, and the partial half llfe is at least thirty-two-
fold greater than that calculated. It is significant that there is other evidence
(68, 105) that the first excited state of ~°~ is nota ro ta tional stat e. Here, it
seems, is a presently isolated but important item which must be included in
a comprehensive a-decay theory. If we may generalize from this single case,
we may postulate that a 2+ state of an even-even nucleus is populated
"normally" only if it is a collective state of the type discussed.
The examination of transitions to the 4+ state gives a totally different
and unique picture (106). Here, if the partial half lives are calculated
above, it is found that they are much shorter than the measured values;
that is, the 4+ states are populated much more sparsely than would be ex-
pected on the basis of a-energy alone. Furthermore, the ratio of measured
half life to calculated half life varies considerably and in a more or less
regular way with atomic number as shown in Figure 11. It is seen that for
Cm ~4~ the second even state is hindered in its population by a factor of 400
(compare with factor 1.7 for first even state, Table III), while for Th isotopes
this factor is of the order of 10. There is no a priori justification for plotting
the data of Figure 11 in the manner shown; for the present it merely serves
the purpose of giving visual expression to the considerable range encoun-
tered in the population of apparently identical spectroscopic states.
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184 PERLMAN AND ASARO


IOOC
oALPHA PARTICLE SPECTROGRAPH DATA
x GAMMA RAY DATA
242
Crn

~Cf246
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I00 240
~pu

0232
u234~ J
Th228o U--~,/
I0 230
Th230...Q.~.~ ¯ U

, I ., I., I I, | I
88 90 92 94 96 98 i00
ATOMIC NUMBER OF PARENT
FIG. 11. Departurefactors for (z-groups to the second
even spin state of even-evennuclides.

Recently, an attack has been made on this problem which appears fruit-
ful. The basic idea developed by Preston (107) is that the e-particle emerging
through the coulomb potential region and beyond the range of nuclear forces
can couple ~vith a noncentral electric field of the nucleus in such a way as to
change its energy. Such fields would be associated with spheroidal distortions
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ALPHA RADIOACTIVITY 185

in nuclei as discussed by Bohr & Mottelson (68) and Hill & Wheeler (108).
The distortion would be described by the intrinsic quadrupole momentwhich
Ford (69) has shown by calculations to be increasing with mass number
the region above Pb and would presumably continue until the approach to a
newshell is felt.
The mechanism of quadrupole interaction with the emerging a-particle
wave to explain the population of the first two excited states in a rotational
band has been explored in detail by Rasmussen (109). For the case of ~4~
decay, for which approximate numerical integrations have been carried out
(assuming an intrinslc quadrupole moment, Q0, in Pu~3~ of + 17 X 10-~ cm3),
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he found that the population of the 2 + state should be relatively unaffected,


but that the population of the 4+ state should be strongly depressed in es-
sential agreement with the experimental observations. The assumed value
for Q0 seems reasonable for a nucleus in this region in view of the recent
measurement of the quadrupole moment of U~35 as +8X10-~4 cm3 (112),
which with the spin of 5/2 corresponds to a value for Qo of +22 X10-34 2. cm.
The quadrupole moment for even-even nuclei cannot, of course, be measured
by spectroscopic means, but there is the possibility of obtaining information
through coulomb excitation cross sections and 3’-ray lifetimes.
Since this approach in explaining certain features of a-spectra is in an
incomplete state of development, it is not worthwhile to speculate on the
possible significance of the downturn of the curve of Figure 11 between
Cm~a and Cf~4~, nor to discuss a number of other ramifications of the mecha-
nism.
Weshall just recall that other low-lying states in even-even nuclei have
been identified, but for which detailed information is lacking. There is the
third even state (6+?) which is a member of the well-defined rotational
band. Also, in a limited region there appear 1- states which are populated
roughly to the same extent as the 4+ states in the same region. It is not clear
what type of nuclear configuration would give rise to such states.
Odd nucleon alpha emitters.--The most obvious question concerning this
category of a-emitters is why the ground state transition is often highly
hindered and why the hindrance is so irregular. Table IV shows the data for
such a-emitters and the last column contains the "departure factor" which,
as before, is the ratio of the measured partial half life for a transition to the
half life which would be calculated from one body a-decay theory. Wenote
that for the four species shown in Figure 8 the departure factors for the ap-
parent ground state transitions are: U2~8--1.4, Am~41--1000, Am*~5--700,
Cm~--->26. It is not certain that for each case in Table IV the ground
state transition has been identified and where this should prove to be the
case the departure factor would be larger.
The first point to be disposed of is the effect of spin change. As already
pointed out in a number of instances, both theoretical and experimental ap-
praisal indicates that the Ill.crime iS relatively insensitive to spin change, .per
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186 PERLMAN AND ASARO


TABLE IV
POPULATION OF GROUND STATE BY ALPHA DECAY OF ODD-NUCLEON EMITTERS

Alpha Particle Departure


energy* Abundance t
emitter ’ factor:~

m
Cf 6.00 0.10 300
m
Bk 6.33 0.18 700
~aa
Bk 6.72 0.30 900
Cmm 6.049 < 0.5 > 26
u3
Am 5.341 ~: 0.003 ~ 1000
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~41
Am 5.535 0.0034 700
~a
Pu 5.01 <0.11 >30
~9
Pu 5.150 0.69 3
2~7
Np 4.86 <0.15 >50
9~
U 4.58 0.10 900
~a
U 4.823 0.83 1.4
m
Pa 5.042 0.11 220
n9
Th 5.02 0.10 100
m
Th 6.030 0.19 130
m
Ra 5. 730 0.09 50
*n
Fr 6.409 0.37 10
*t~
Em 6.824 0.69 18
m
Em 5.847 0.33 8
m
At 5. 862 1.00 3

At 5.519 0.32 2
~s
Po 8.336 I. 5
Pom 7.434 0.99 100
~°~
Po 4. 877 2

* Particle energy of a-group believed to lead to the groundstate. In someinstances


it is possible that the groups selected are not the ground state transitions in which
eases the "departure factors" would be greater than those shown.
~ Abundancesare based on observed a-groups except where the highest energy
group is knownto be followed by 3,-radiation.
~t Definedin Table III.

se, certainly within the framework of reasonable spin changes. Conversely,


we know that the ground states of Am~*~ and Np*~r both have spin 5/2 (110,
111) yet the transition between these states is hindered 1000 fold.
Other ideas, not yet formulated quantitatively, appear to be more prom-
ising. One suggestion (31) has to do with the breakdown of the one body
model in its implication that a-particles exist as discrete entities within the
nucleus and that the probabili Wof a-emission depends only upon the fre-
quency factor of this preformed a-particle in encountering the coulomb
barrier and upon the rate of barrier penetration. We have seen that for
ground state transitions of even-even nuclei the evidence for this extreme
simplification indicates that it is substantially correct. For ground state
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ALPHA RADIOACTIVITY 187


transitions of odd nucleon emitters, however,it is suggested (31) that there
can be a considerable time involved in assembling the componentsof the
a-partlcle. Suchwould be the description if the mixture of configurations
which constitutes the emitting nucleus contained only as a minor component
the configuration with the odd particle as a constituent of an incipient a-
particle. Rasmussen(90) has pointed out further that nuclear spins need not
give a true picture of the nucleon states of the parent and daughter nuclei,
In a region well awayfrom a closed shell where large spheroidal distortions
are expected, the strong-coupling configurations maypredominate and the
nuclear spin can be different from and lower than the j-value for the single
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odd nucleon. On this basis, the spectroscopic state of the odd proton in
Am ~41 maybe quite different from that in Np~37 even though both nuclear
spins are 5/2. If such were the case, the change in wavefunctions could
properly introduce a hindrance to the a-decay. Only for those transitions
where the single particle wavefunction remains unaltered wouldone expect
unhindered a-decay. Significantly, it appears that such transitions can be
found in the spectra of the odd nucleon emitters, but in general these are
not the ground state transitions. This subject will nowbe examined.
In Figure 8 it is seen that the most abundant groups of Am ~l ~4~
and Am
lead to states which are 60 and 75 key respectively above the ground state.
Furthermore,for the particular energies of these a-transltions, the hindrance
or departurefactors are only of the order of unity (in contrast to 1000for the
groundstate transitions) and, in this respect, appear to be like the ground
state transitions of even-even nuclei. By makingcertain assumptions it is
possible to deducethe spins for these excited states (60 and 75 key states).
The analysis has already been carried out on page 178 and is based on the
recognition of three excited states as membersof a rotational band from
which the spins of these states can be deduced. In this case, the spins for
the 60 key excKedstate of Np~7 and the 75 key state for Am ~.3 are deduced
to be 5/2 (14, 90). It is suggested (90) then that these states maybe those
which the odd particle wave function rearrangement is a minimumand that
the transition is therefore relatively unhindered.
As already discussed under even-even nuclei, the splitting of a-groups
into a rotational spectrummayinvolve the effect of electric field interactions.
The appearance of what looks like rotational bands in these odd nucleon
species implies, of course, that the same mechanism is in play here.
It seems apparent that the past few years have seen a departure from
classical a-decay theory as well as a reinforcementin our confidencein some
of its aspects. It also seems likely that someof the newideas whenfurther
developed will add appreciably to the explanation of the a-decay process,
and that the ramifications of these ideas wiil provide a better understanding
of nuclear structure.
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188 PERLMAN AND ASARO


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ALPHA RADIOACTIVITY 189

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190 PERLMAN AND ASARO


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